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Mixed Organic Counterion Strategy Modulates the Self-Assembly of Polyoxometalate Hybrids into Toroids and Affects Their Photochromic and Photocatalytic Properties

反离子 多金属氧酸盐 化学 光致变色 混合的 光化学 离子 催化作用 有机化学 植物 生物
作者
Aranya Kar,Chullikkattil P. Pradeep
出处
期刊:Inorganic Chemistry [American Chemical Society]
卷期号:61 (50): 20561-20575 被引量:5
标识
DOI:10.1021/acs.inorgchem.2c03395
摘要

A series of five mixed-counterion polyoxometalate (POM) hybrids 1-5 have been developed starting from the [SiW12O40]4- cluster and two different aryl sulfonium counterions (ASCIs), (4-hydroxyphenyl)dimethylsulfonium (HPDS) and (4-formylphenyl)dimethylsulfonium (FPDS), bearing different functional groups -OH and -CHO, respectively. The HPDS/FPDS counterion ratio in hybrids 1-5 varied as 4:0 (1), 3:1 (2), 2:2 (3), 1:3 (4), and 0:4 (5), and it resulted in a morphological transition of the self-assembly of these hybrids. Hybrid 1 exhibited spherical self-assembly, while hybrid 5 exhibited large toroidal self-assembly predominantly. The hybrids 2-4 gave a mixture of spherical, dimpled spherical, and toroidal self-assemblies in varying amounts, indicating a gradual transition of self-assembly from spherical to toroidal as the percentage of FPDS increases in the system. A plausible explanation for the differences in the self-assembly properties of these hybrids has been proposed based on the differences in the H-bonding interactions of the two counterions with the dispersion medium. The HPDS and FPDS counterions exhibited different HOMO-LUMO gaps, and their varying percentages in hybrids 1-5 led to differences in optical band gaps and photochromic activities. Hybrid 2 showed the lowest band gap value and the best photochromic activity (t1/2 = 0.72 min) in the series. The influence of the mixed-counterion strategy in catalysis has been demonstrated by evaluating the photocatalytic activity of these hybrids toward rhodamine B dye degradation. The hybrid 4, exhibiting stable toroidal self-assembly, showed the best catalytic activity in the series, probably due to a combination of reasons such as the enhanced surface area due to toroid formation and also the presence of H-bonding -OH functionality on the counterion. Therefore, the present study suggests a new method for altering the self-assembly and the materials and catalytic properties of POM hybrids through a mixed-counterion strategy.
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